Fluxes of lead to the Great Lakes are dominated by atmospheric depositions of industrial lead, which account for ~ 64% of the lead inputs to Lake Ontario and >90% of the inputs to Lake Superior. It has recently been demonstrated that lead aerosols in the Great Lakes region may be identified by the contrasting 206Pb/207Pb ratios of industrial leads from the United States (1.221 ±0.009) and Canada (1.151 ±0.010). Here we show that those ratios may also be used to identify and trace industrial lead inputs to the Great Lakes. These corroborate spatial gradients in lead concentrations in surface waters, which range from 290 pmol kg−1 in Hamilton Harbour to <10 pmol kg−1 in the central waters of Lake Ontario. The latter concentrations and corresponding residence-time estimates, which are both an order of magnitude lower than previously reported, indicate that lead is rapidly scavenged in the epilimnion during periods of high primary productivity. We find that industrial lead from Canada and the United States are the two principal sources of lead contamination in the Great Lakes.